We study a system of a transition metal dichalcogenide (TMD) monolayer placed in an optical resonator, where strong light-matter coupling between excitons and photons is achieved. We present quantitative theory of the nonlinear optical response for exciton-polaritons for the case of doped TMD monolayer, and analyze in detail two sources of nonlinearity. The first nonlinear response contribution stems from the Coulomb exchange interaction between excitons. The second contribution comes from the reduction of Rabi splitting that originates from phase space filling at increased exciton concentration and the composite nature of excitons. We demonstrate that both nonlinear contributions are enhanced in the presence of free electrons. As free electron concentration can be routinely controlled by an externally applied gate voltage, this opens a way of electrical tuning of the nonlinear optical response.
The spin Hall effect for polaritons (SHEP) in a transition metal dichalcogenides (TMDC) monolayer embedded in a microcavity is predicted. We demonstrate that two counterpropagating laser beams incident on a TMDC monolayer can deflect a superfluid polariton flow due to the generation the effective gauge vector and scalar potentials. The components of polariton conductivity tensor for both non-interacting polaritons without Bose-Einstein condensation (BEC)and for weakly-interacting Bose gas of polaritons in the presence of BEC and superfluidity are obtained. It is shown that the polariton flows …
The resonant scattering of surface plasmon-polariton waves by embedded semiconductor quantum dots above the dielectric/metal interface is explored in the strong-coupling regime. In contrast to non-resonant scattering by a localized dielectric surface defect, a strong resonant peak in the scattering field spectrum is predicted and accompanied by two side valleys. The peak height depends nonlinearly on the amplitude of surface plasmon-polariton waves, reflecting the feedback dynamics from a photon-dressed electron-hole plasma inside the quantum dots. This unique behavior in the scattering field …
While conventional semiconductor technology relies on the manipulation of electrical charge for the implementation of computational logic, additional degrees of freedom such as spin and valley offer alternative avenues for the encoding of information. In transition metal dichalcogenide (TMD) monolayers, where spin-valley locking is present, strong retention of valley chirality has been reported for MoS$_2$, WSe$_2$ and WS$_2$ while MoSe$_2$ shows anomalously low valley polarisation retention. In this work, chiral selectivity of MoSe$_2$ cavity polaritons under helical excitation is reported wi…
Polaritons, mixed light-matter quasiparticles, undergo a transition to a condensed, macroscopically coherent state at low temperatures or high densities. Recent experiments show that coupling light to organic molecules inside a microcavity allows condensation at room temperature. The molecules act as saturable absorbers with transitions dressed by molecular vibrational modes. Motivated by this we calculate the phase diagram and spectrum of a modified Tavis-Cummings model, describing vibrationally dressed two-level systems, coupled to a cavity mode. Coupling to vibrational modes can induce re-e…
Strong coupling between light and matter is possible with a variety of organic materials. In contrast to the simpler inorganic case, organic materials often have a complicated spectrum, with vibrationally dressed electronic transitions. Strong coupling to light competes with this vibrational dressing, and if strong enough, can suppress the entanglement between electronic and vibrational degrees of freedom. By exploiting symmetries, we can perform exact numerical diagonalization to find the polaritonic states for intermediate numbers of molecules, and use these to define and validate accurate e…
We study the collective, superradiant behavior in the system of emitter-dressed Ag nanorods. Starting from the Drude model for the plasmon oscillations, we arrive at a semi-empirical Hamiltonian describing the coupling between quantized surface plasmon modes and the quantum emitters that can be controlled by manipulating their geometry, spacing, and orientation. Further, identifying the lowest polariton mode as SP-states dressed by excitons in the vicinity of $k=0$, we examine conditions allowing for the polariton quantum phase transition. While the system is formally a 1D array, we show that …
Atomically thin transition metal dichalcogenides (TMDs) possess a number of properties that make them attractive for realizing room-temperature polariton devices. An ideal platform for manipulating polariton fluids within monolayer TMDs is that of Bloch surface waves, which confine the electric field to a small volume near the surface of a dielectric mirror. Here we demonstrate that monolayer tungsten disulfide ($\text{WS}_2$) can sustain Bloch surface wave polaritons (BSWPs) with a Rabi splitting of 43 meV and propagation constants reaching 33 $μ$m. In addition, we evidence strong polariton-p…
Keldysh field theory of spin- and valley-distinguished polariton nonlinearities in transition-metal dichalcogenide monolayers
Abrikosov Center for Theoretical Physics, Moscow Center for Advanced Studies（阿布里科索夫理论物理中心，莫斯科高等研究中心）；National Research Nuclear University MEPhI (Moscow Engineering Physics Institute)（国立研究核大学MEPhI（莫斯科工程物理学院））；Russian Quantum Center, Skolkovo IC（俄罗斯量子中心，斯科尔科沃创新中心）
We study the coherent properties of plasmon polaritons optically excited on periodic nanostructures. The gold grains are coupled to a single mode photonic waveguide which exhibits a dramatically reduced transmission originating from the derived quantum interference. With a nonequilibrium description of Floquet-dressed polaritons we demonstrate the switching of light transmission through the waveguide due to sheer existence of intraband transitions in gold from right above the Fermi level driven by the external laser light.
A monolayer of transition metal dichalcogenide (TMDC) is shown to be capable of supporting a guided optical mode below the exciton resonance, a two-dimensional exciton polariton. This visible or near IR mode is confined roughly within a micrometer from the monolayer and has propagation length exceeding 100 micrometers. The light guiding ability makes TMDC monolayers more versatile and potentially attractive photonic platform.
Atomically-thin transition metal dichalcogenide crystals (TMDCs) hold great promise for future semiconductor optoelectronics due to their unique electronic and optical properties. In particular, electron-hole pairs (excitons) in TMDCs are stable at room temperature and interact strongly with light. When TMDCs are embedded in an optical microcavity, the excitons can hybridise with cavity photons to form exciton polaritons (polaritons herein), which display both ultrafast velocities and strong interactions. The ability to manipulate and trap polaritons on a microchip is critical for future appli…
Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form quasiparticles known as polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with cavity-assisted hyperspectral imaging. Using extended WS$_2$ monolayers, we establish the regime of strong coupling with a scanning microcavity to map out polariton pro…
Transition metal dichalcogenide (TMD) monolayers are direct bandgap semiconductors that feature tightly bound excitons, strong spin-orbit coupling, and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a new method for probing the optical properties of two-dim…
The monolithic integration of electronics and photonics has attracted enormous attention due to its potential applications. However, the realization of such hybrid circuits has remained a challenge because it requires optical communication at nanometer scales. A major challenge to this integration is the identification of a suitable material. After discussing the material aspect of the challenge, we identified atomically thin transition metal dichalcogenides (TMDs) as a perfect material platform to implement the circuit. The selection of TMDs is based on their very distinct property: monolayer…
We calculate the dispersion of spinor exciton-polaritons in a planar microcavity with its active region containing a single Transitional Metal Dichalcogenide (TMD) monolayer, taking into account excitonic and photonic spin-orbit coupling. We consider the radial propagation of polaritons in presence of disorder. We show that the reduction of the disorder scattering induced by the formation of polariton states allows to observe an optical Valley Hall effect, namely the coherent precession of the locked valley and polarization pseudospins leading to the formation of spatial valley-polarized domai…
We describe a mechanism by which an electrical bias voltage applied across a unipolar semiconductor quantum well can drive an exciton or polariton supercurrent. The mechanism depends on the properties of electronic quasiparticles in quantum wells or two-dimensional materials that are dressed by interactions with the coherent exciton field of an exciton condensate or the coherent exciton and photon fields of a polariton condensate, and on approximate conservation laws. We propose experiments that can be performed to realize this new light-matter coupling effect, and discuss possible application…
Recently reported large values of exciton-polariton nonlinearity of transition metal dichalcogenide (TMD) monolayers coupled to optically resonant structures approach the values characteristic for GaAs-based systems in the regime of strong light-matter coupling. Contrary to the latter, TMD-based polaritonic devices remain operational at ambient conditions and therefore have greater potential for practical nanophotonic applications. Here we present the study of the nonlinear properties of Ta$_2$O$_5$ slab waveguide coupled to a WSe$_2$ monolayer. We first confirm that the hybridization between …
We present a microscopic theory of the equilibrium polariton condensate state of a semiconductor quantum well in a planar optical cavity. The theory accounts for the adjustment of matter excitations to the presence of a coherent photon field, predicts effective polariton-polariton interaction strengths that are weaker and condensate exciton fractions that are smaller than in the commonly employed exciton-photon model, and yields effective Rabi coupling strengths that depend on the detuning of the cavity photon energy relative to the bare exciton energy. The dressed quasiparticle bands that app…
Two-dimensional transition metal dichalcogenide (TMD) semiconductors provide a unique possibility to access the electronic valley degree of freedom using polarized light, opening the way to valley information transfer between distant systems. Excitons with a well-defined valley index (or valley pseudospin) as well as superpositions of the exciton valley states can be created with light having circular and linear polarization, respectively. However, the generated excitons have short lifetimes (ps) and are also subject to the electron-hole exchange interaction leading to fast relaxation of the v…
Excitons, composite electron-hole quasiparticles, are known to play an important role in optoelectronic phenomena in many semiconducting materials. Recent experiments and theory indicate that the band-gap optics of the newly discovered monolayer transition-metal dichalcogenides (TMDs) is dominated by tightly bound valley excitons. The strong interaction of excitons with long-range electromagnetic fields in these 2D systems can significantly affect their intrinsic properties. Here, we develop a semi-classical framework for intrinsic exciton-polaritons in monolayer TMDs that treats their dispers…
Semiconducting transition-metal dichalcogenides (TMDCs) provide a fascinating discovery platform for strong light-matter interaction effects in the visible spectrum at ambient conditions. While most of the work has focused on hybridizing excitons with resonant photonic modes of external mirrors, cavities, or nanostructures, intriguingly, TMDC flakes of sub-wavelength thickness can themselves act as nanocavities. Here, we determine the optical response of such freestanding planar waveguides of WSe$_2$, by means of cathodoluminescence spectroscopy. We reveal strong exciton-photon interaction eff…
Monolayer (ML) transition metal dichalcogenides (TMDs) integrated in optical microcavities host exciton-polaritons as a hallmark of the strong light-matter coupling regime. Analogous concepts for hybrid light-matter systems employing spatially indirect excitons with a permanent electric dipole moment in heterobilayer (HBL) crystals promise realizations of exciton-polariton gases and condensates with immanent dipolar interactions. Here, we identify optical signatures of spatially indirect momentum-bright and momentum-dark interlayer excitons in vertical MoSe$_2$-WSe$_2$ heterostructures and imp…
We present a theory of the cavity quantum electrodynamics of the graphene cyclotron resonance. By employing a canonical transformation, we derive an effective Hamiltonian for the system comprised of two neighboring Landau levels dressed by the cavity electromagnetic field (integer quantum Hall polaritons). This generalized Dicke Hamiltonian, which contains terms that are quadratic in the electromagnetic field and respects gauge invariance, is then used to calculate thermodynamic properties of the quantum Hall polariton system. Finally, we demonstrate that the generalized Dicke description fail…
Highly nonlinear optical materials with strong effective photon-photon interactions (Kerr-like nonlinearity) are required in the development of novel quantum sources of light as well as for ultrafast and quantum optical signal processing circuitry. Here we report very large Kerr-like nonlinearities by employing strong optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe$_2$ at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at…
The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. One promising platform to reach such strong light-matter interacting regimes is offered by polaritonic metasurfaces, which represent ultrathin artificial media structured on nano-scale and designed to support polaritons - half-light half-matter quasiparticles. Topological polaritons, or 'topolaritons', offer an ideal platform in this context, with unique properties stemming from topological phases of…
The newly discovered valley degree of freedom in atomically thin two-dimensional transition metal dichalcogenides (TMD) offers a promising platform to explore rich nonlinear physics, such as spinor Bose-Einstein condensate (BEC) and novel valleytronics applications. However, the critical nonlinear effect, such as valley polariton bosonic stimulation, has long remained an unresolved challenge due to the generation of limited polariton ground state densities necessary to induce the stimulated scattering of polaritons in specific valleys. Here, we report the self-induced valley bosonic stimulatio…
Two-dimensional transition metal dichalcogenides (TMDCs) have recently become attractive semiconductor materials for several optoelectronic applications, such as photodetection, light harvesting, phototransistors, light-emitting diodes, and lasers. They are particularly appealing because their bandgap lies in the visible and near-IR range, and they possess strong excitonic resonances, high oscillator strengths, and valley-selective response. Coupling these materials to optical nanocavities enhances the quantum yield of exciton emission, enabling advanced quantum optics and nanophotonic devices…
The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional (2D) transition metal dichalcogenide (TMDC) deposited onto a metal substrate or coating a metallic thin-film. We determine the polaritonic spectrum and show that, in the former case, the addition of a top dielectric layer, and, in the latter, the thickness of the metal film,can be used to tune and promote plasmon-exciton interactions well within the strong coupling re…
In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride (hBN), low-loss infrared-active phonon-polaritons exhibit hyperbolic behavior for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transitio…
Van der Waals materials and heterostructures manifesting strongly bound room temperature exciton states exhibit emergent physical phenomena and are of a great promise for optoelectronic applications. Here, we demonstrate that nanostructured multilayer transition metal dichalcogenides by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of excitons and hybrid polaritons with interaction potentials exceeding 410 meV may be …
Electric dipole transitions between different cavity polariton branches or between dressed atomic states with the same excitation number are strictly forbidden in centro-symmetric systems. For doped quantum wells in semiconductor microcavities, the strong coupling between an intersubband transition in the conduction band and a cavity mode produces two branches of intersubband cavity polaritons, whose normal-mode energy splitting is tunable and can be in the terahertz region. Here, we show that, by using asymmetric quantum wells, it is possible to have allowed dipolar transitions between differ…
Dirac plasmons in graphene hybridize with phonons of transition metal dichalcogenides (TMDs) when the materials are combined in so-called van der Waals heterostructures (vdWh), thus forming surface plasmon-phonon polaritons (SPPPs). The extend to which these modes are coupled depends on the TMD composition and structure, but also on the plasmons' properties. By performing realistic simulations that account for the contribution of each layer of the vdWh separately, we calculate how the strength of plasmon-phonon coupling depends on the number and composition of TMD layers, on the graphene Fermi…
Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling strength, and probed by a time domain 2DIR technique, Double Quantum Coherence (DQC). Applications are made to the amide-I ($CO$) and amide-II ($CN$) bond vibrations of $N-methylacetamide$ (NMA).
Emergence of Propagating Exciton-Polaritons in Hybrid Waveguide-van der Waals Heterostructures
Institute of Physics, University of Rostock（罗斯托克大学物理研究所）；Ferdinand-Braun-Institut, Leibniz-Institut für Höchstfrequenztechnik (FBH)（费迪南德·布劳恩研究所，莱布尼茨高频技术研究所）；Research Center for Materials Nanoarchitectonics, NIMS（日本物质材料研究机构纳米结构材料研究中心）；Research Center for Electronic and Optical Materials, NIMS（日本物质材料研究机构电子光学材料研究中心）
Electrically reconfigurable dipolar polaritons with highly tunable nonlinearity in a homobilayer microcavity
Tsinghua University（清华大学）；University of Washington（华盛顿大学）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；National Institute for Materials Science（国立材料研究所）；Nanyang Technological University（南洋理工大学）；Frontier Science Center for Quantum Information（量子信息前沿科学中心）
The interaction of organic molecules and molecular aggregates with electromagnetic fields that are strongly confined inside optical cavities within nanoscale volumes, has allowed the observation of exotic quantum regimes of light-matter interaction at room temperature, for a wide variety of cavity materials and geometries. Understanding the universal features of such organic cavities represents a significant challenge for theoretical modelling, as experiments show that these systems are characterized by an intricate competition between coherent and dissipative processes involving entangled nuc…
While photons in vacuum are massless particles that do not interact with each other, significant photon-photon interactions appear in suitable nonlinear media, leading to novel hydrodynamic behaviors typical of quantum fluids. Here we show the formation of vortex-antivortex pairs in a Bose-Einstein condensate of exciton-polaritons -a coherent gas of strongly dressed photons- flowing at supersonic speed against an artificial potential barrier created and controlled by a light beam in a planar semiconductor microcavity. The observed hydrodynamical phenomenology is in agreement with original theo…
We study a 2D system of trion-polaritons at the quantum level and demonstrate that for monolayer semiconductors they can exhibit a strongly nonlinear optical response. The effect is due to the composite nature of trion-based excitations resulting in their nontrivial quantum statistical properties, and enhanced phase space filling effects. We present the full quantum theory to describe the statistics of trion-polaritons, and demonstrate that the associated nonlinearity persists at the level of few quanta, where two qualitatively different regimes of photon antibunching are present for weak and …
We investigate the many-body states of exciton-polaritons that can be observed by pump-probe spectroscopy. Here, a weak-probe `spin-down' polariton is introduced into a coherent state of `spin-up' polaritons created by a strong pump. We show that the $\downarrow$ impurities become dressed by excitations of the $\uparrow$ medium, and form new polaronic quasiparticles that feature two-point and three-point many-body quantum correlations, which, in the low density regime, arise from coupling to the vacuum biexciton and triexciton states respectively. In particular, we find that these correlations…
Atomically thin semiconductors such as transition metal dichalcogenide (TMD) monolayers exhibit a very strong Coulomb interaction, giving rise to a rich exciton landscape. This makes these materials highly attractive for efficient and tunable optoelectronic devices. In this article, we review the recent progress in the understanding of exciton optics, dynamics and transport, which crucially govern the operation of TMD-based devices. We highlight the impact of hBN-encapsulation, which reveals a plethora of many-particle states in optical spectra, and we outline the most novel breakthroughs in t…
Two dimensional (2D) semiconductor materials of transition-metal dichalcogenides (TMDCs) manifest many peculiar physical phenomena in the light-matter interaction. Due to their ultrathin property, strong interaction with light and the robust excitons at room temperature, they provide a perfect platform for studying the physics of strong coupling in low dimension and at room temperature. Here we report the strong coupling between 2D semiconductor excitons and Tamm plasmon polaritons (TPPs). We observe a Rabi splitting of about 54 meV at room temperature by measuring the angle resolved different…
Systems with strong light-matter interaction opens up new avenues for studying topological phases of matter. Examples include exciton-polaritons, mixed light-matter quasiparticles, where the topology of the polaritonic band structure arises from the collective coupling between matter wave and optical fields strongly confined in periodic dielectric structures. Distinct from light-matter interaction in a uniform environment, the spatially varying nature of the optical fields leads to a fundamental modification of the well-known optical selection rules, which were derived under the plane wave app…
The two-dimensional transition-metal dichalcogenides (2D TMDCs) are an intriguing platform for studying light-matter interactions because they combine the electronic properties of conventional semiconductors with the optical resonances found in organic systems. However, the coupling strengths demonstrated in strong exciton-polariton coupling remain much lower than those found in organic systems. In this paper, we take on a new approach by utilizing the large oscillator strength of the above-band gap C exciton in few-layer molybdenum disulphide ($\text{FL-MoS}_2$). We show a k-space Rabi splitt…
Strong light-matter interactions between resonantly coupled metal plasmons and spin decoupled bright excitons from two dimensional (2D) transition metal dichalcogenides (TMDs) can produce discrete spin-resolved exciton-plasmon polariton (plexciton). A few efforts have been made to perceive the spin induced exciton-polaritons in nanocavities at cryogenic conditions, however, successful realization of spin-resolved plexciton in time-domain is still lacking. Here, we are able to identify both the spin-resolved plexcitons discretely at room temperature and investigate their ultrafast temporal dyna…
We present a microscopic semi-analytical theory for the description of organic molecules interacting strongly with a cavity mode. Exciton-vibration coupling within the molecule and exciton-cavity interaction are treated on an equal footing by employing a temperature-dependent variational approach. The interplay between strong exciton-vibration coupling and strong exciton-cavity coupling gives rise to a hybrid ground state, which we refer to as the lower polaron polariton. Explicit expressions for the ground-state wave function, the zero-temperature quasiparticle weight of the lower polaron pol…
The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observ…
Spin-orbit coupling is a fundamental mechanism that connects the spin of a charge carrier with its momentum. Likewise, in the optical domain, a synthetic spin-orbit coupling is accessible, for instance, by engineering optical anisotropies in photonic materials. Both, akin, yield the possibility to create devices directly harnessing spin- and polarization as information carriers. Atomically thin layers of transition metal dichalcogenides provide a new material platform which promises intrinsic spin-valley Hall features both for free carriers, two-particle excitations (excitons), as well as for …
